TW200950174A - Organic electroluminescent element - Google Patents

Abstract

This invention provides an organic electroluminescent element constituted by a laminate in the order of a functional layer, a transparent first electrode, a luminescent layer, and a second electrode. The functional layer has a surface positioned away from the first electrode, which surface has a plurality of undulations having heights from 0.5 μ m to 100 μ m, and the first electrode and the functional layer respectively have refraction indexes of n1 and n2 which satisfy the following formula (1): 0.3 ≥ (n1-n2) ≥ 0...formula (1)

Description

200950174 VI. Description of the Invention: [Technical Field] The present invention relates to an organic electric field light-emitting element, a lighting device, a display device, and a method of manufacturing the same. [Prior Art] An organic electroluminescence (Electro Luminescence) element is composed of a light-emitting layer containing an organic substance and a pair of electrodes containing the light-emitting layer. When a voltage is applied to the organic EL element, electrons can flow from the cathode and the holes can flow from the anode, and the electrons can be combined with the holes in the light-emitting layer to emit light. The light emitted from the light-emitting layer can be obtained from at least one of the pair of electrodes. Therefore, a transparent electrode is used for the electrode of the side where light can be obtained. The transparent electrode is formed of, for example, a metal oxide such as indium tin oxide (ITO: Indium Tin Oxide). Since the refractive index of the metal oxide used in the general transparent electrode is higher than the refractive index of the substrate on which the organic EL element is disposed, total reflection can be generated in the boundary between the transparent electrode and the substrate. Most of the light emitted from the light-emitting layer cannot be obtained outside the organic EL element by such reflection or the like, so that the light-receiving efficiency is inevitably low. Therefore, an organic EL element having a structure capable of suppressing such reflection has been proposed. For example, an organic EL element using a glass substrate on which a light-concentrating concentrating layer is provided is used (for example, refer to Japanese Laid-Open Patent Publication No. 2003-86353). The concentrating layer is formed of a condensing structure such as a micro lens and a transparent resin covering the condensing structure. Among the transparent resins, those having a higher refractive index than the condensing structure are used. When such a light-concentrating layer is provided on the glass substrate, the total anti-321152 3 200950174 shot produced on the surface of the glass substrate can be suppressed to achieve the light-recovering efficiency. I. SUMMARY OF THE INVENTION Even if such a concentrating layer has been provided on a glass substrate, since the total reflection occurs at the interface between the concentrating layer and the glass substrate, the A-rate of light from the organic EL element is not very high. Therefore, it is necessary to seek an organic EL element which is effective in light. @m目=provide: an organic EL element with high light efficiency, a device for displaying the device, and a method for manufacturing the same. The present invention is an organic electric field invention of the basin 1 Leiquan Duyou 70, which is a functional layer, a transparent first electrode, a light-emitting layer and a second electrode of a smoothing electric field light-emitting element, sequentially stacked, and The refractive index n1 of the first electrode having the height of 0.5//ID to 1 第 in the functional layer described above satisfies the following formula (1). On the surface of the opposite side of the electrode, the concave and convex portion of the shape, the refractive index of the functional layer of the moon J η 2 -uu-n~su ·.. (1) Further, the present invention is composed of an organic electric field refractive index layer, which is low. The refractive index layer system is provided with a surface adjacent to the opposite side of the charging electrode. The refractive index n1 of the functional layer and the first first electrode, and the refractive index n3 of the low refractive index layer can satisfy the lower refractive index n2 nl^n2>n3 (2) Further, the present invention is a The organic electric field luminescence is a % member, wherein the center line average roughness Ra of the surface of the first electrode side of the energy layer of the device is 21 nm or less. 5至该至100//米。 The present invention is an organic electroluminescent device, wherein the arrangement of the concave and convex portions is 0. 5 / im to 100 / / m. Further, the present invention is an organic electroluminescence device in which the surface shape of each of the uneven portions is a concave surface or a convex surface. Further, the present invention is an organic electroluminescence element in which the concave or convex surface is a hemispherical surface. Further, the present invention is an organic electroluminescence device in which the surface shapes of the respective concavities and convexities are each composed of a plurality of planes. Further, the present invention is an organic electric field light-emitting element in which the shape of the concave and convex portions is irregular to each other. Meanwhile, the present invention is an illumination device including the above organic electric field light-emitting element. Meanwhile, the present invention is a φ display device including a plurality of the above-described organic electric field light-emitting elements. Moreover, the present invention is a method for producing an organic electroluminescence device, which is composed of a low refractive index layer, a functional layer, a transparent first electrode, a light-emitting layer and a second electrode, and is composed of the first electrode. The refractive index n1, the refractive index n2 of the functional layer, and the refractive index n3 of the low refractive index layer satisfy the following formula (3), 0. 3^(nl - n2)^, < · · · (3) nl ^n2>n3 This method includes the steps of forming a plurality of low refractive index layers having a plurality of heights of 0.5/m to 100 5 321152 200950174 /zm; and forming the aforementioned low refractive index layer a step of forming a functional layer after coating a coating liquid containing a material as a functional layer on the surface of the uneven portion; a step of forming a first electrode; a step of forming a light-emitting layer; and a step of forming a second electrode. Further, the present invention is a method for producing an organic electroluminescence device, in which a plurality of concave and convex portions are formed by an imprinting method in the step of forming the low refractive index layer. Moreover, the present invention is a method of fabricating an organic electroluminescence device. In the step of forming the low refractive index layer, a plurality of irregularities are formed by selectively removing a surface portion of the low refractive index plate by a lithography technique. Part. Further, the present invention is a method for producing an organic electroluminescence device, in which the surface portion of the low refractive index plate is selectively removed by a dry etching technique in the step of forming the low refractive index layer to form an uneven portion. [Embodiment] FIG. 1 is a schematic view showing an organic electroluminescence device (hereinafter also referred to as an organic EL device) 1 according to an embodiment of the present invention. The organic EL element 1 is composed of at least a low refractive index layer 2, a functional layer 3, a transparent first electrode 4, a light-emitting layer 5, and a second electrode 6 laminated in this order. On the surface of the functional layer 3 opposite to the first electrode, a plurality of concave and convex portions having a height of 0.5 Am to 100 / / m are formed. Further, the refractive index n1 of the first electrode and the refractive index n2 of the functional layer satisfy the following formula (1). 6 321152 200950174 0.3^ (nl-n2) ^ 0 (1) and the refractive index η of the first electrode, the refractive index η2 of the functional layer, and the refractive index n3 of the low refractive index layer satisfy the following formula (2) ). η 1 2 > n 3 ·*·(2) The first electrode 4 and the second electrode 6 are not limited to one layer of the light-emitting layer 5, and a plurality of light-emitting layers may be provided, and/or with the light-emitting layer. Different layers or multiple layers. In the organic EL element 1 of the present embodiment, a hole injection layer 7 is provided between the first electrode 4 and the light-emitting layer 5. The low refractive index layer 2 is provided adjacent to the surface of the functional layer 3 opposite to the first electrode 4. In the present embodiment, the laminate of the low refractive index layer 2 and the functional layer 3 has a function as the substrate 8. The organic EL element 1' of the present embodiment is composed of a substrate 8 , a first electrode 4, a hole injection layer 7, a light-emitting layer 5, and a second electrode 6 which are adjacent to each other. Meanwhile, in the present embodiment, the substrate 8 is adjacent to the first electrode 4, but a thin insulating layer or a barrier layer may be provided between the substrate 8 and the first electrode 4, for example. The first electrode 4 of the present embodiment can exhibit transparency and function as an anode, and the second electrode 6 can reflect visible light and has a function as a cathode. The substrate 8 is shown to have transparency. Therefore, the light emitted from the light-emitting layer 5 to the first electrode 4 passes through the first electrode 4 and the substrate 8, and is then taken outside. The light emitted from the light-emitting layer 5 to the second electrode 6 is reflected by the second electrode 6, and is received by the first electrode 4 and the substrate 8 on the outside. That is, the organic component element of the present embodiment is a bottom emission type element that obtains light from the substrate 8. 7 321152 200950174 In a modification, a bottom emission plastic organic EL element having a first electrode as a cathode and a second electrode as an anode may be formed, or a light transmissive electrode may be used on the second electrode, and the composition may be An organic EL element that double-lights the light while obtaining the second electrode. Since the refractive index of the functional layer 3 and the first electrode 4 represented by the formula (1) is small, the reflection in the interface between the functional layer 3 and the first electrode 4 can be made low, and the total reflection can be suppressed. . Thereby, the wire can be efficiently transferred from the 1 electrode 4 to the functional layer 3. To: a plurality of heights 〇5^ and a low-refraction shirt 2^4 can be formed on the surface of the functional layer 3, thereby suppressing the functional layer 3 "light: reflection in the surface, and the first electrode 4 The ^7 of the incident W portion is incident on the low refractive index layer 2 by an effective person. The drum is good at each time. The two "G·7#"1 to 50_' and even 30_. Further, the weight is perpendicular to the height of each uneven portion in the direction of the first electrode 4 of the functional layer 3. 1 electrode 4 side table The heat and groove referred to herein is measured by the device. . Further, the "degree" usable stylus type concavity and convexity is as shown in the formula (2), and the refractive index of the low refractive index 2 plate 4 and the functional layer 3 is lower than the refractive index of the first electrical, so, the ratio of the functional layer 3 is closer to the empty ~: the total reflection generated on the interface, and inflammation, because the 彳 1 1 is effective in the outer peak. Into a ^ please _ = Γ air interface on the formation of a plurality of concave and convex parts of height 0·5, Therefore, the light having the lower refractive index of 321152 8 200950174 layer 2 can be effectively obtained outside. As described above, the light emitted from the light-emitting layer 5 can be efficiently transferred to the first electrode 4 and the functional layer 3 in order. The low refractive index layer 2 and the air can improve the efficiency of light acquisition. Since the conventional technique is to provide the concentrating structure on the glass substrate, a part of the light can be disposed at the interface between the concentrating layer and the glass substrate. In the organic EL element 1 of the present embodiment, the low refractive index layer 2 having a corresponding structure is incorporated in the concentrating structure of the prior art, and the condensing property in the technique of using the prior art is used. The low refractive index layer 2 in which the structure is integrally formed with the glass substrate has no conventional technique. In the case where reflection occurs at the interface between the concentrating layer and the glass substrate, the efficiency of light acquisition can be improved. The unevenness of the surface of the side of the first electrode 4 of the functional layer 3 is for the layer deposited on the surface of the functional layer 3 The flatness of the first electrode 4 is affected. When the flatness of the first electrode 4 is low, a short circuit occurs due to the protrusion of the first electrode 4. Therefore, the center line average roughness Ra of the first electrode 4 is Preferably, when the first electrode 4 is to be formed, the center line average roughness Ra of the surface of the first electrode 4 of the functional layer 3 is preferably the smaller one. The center line average roughness Ra of the surface of the first electrode 4 of 3 is preferably 100 nm or less, more preferably 50 nm or less, more preferably 1 Ornn or less, still more preferably 3 nm or less. The configuration interval of the copy is, for example, 0.4/z in to 200 /zm, and preferably 0.5·5 m to 100 // m, and preferably 0.80 m to 50 /zm. By arranging the uneven portions at such intervals, the effect of scattering, refraction, and condensing can be made large, and it is expected to improve light-harvesting efficiency. 9 321152 200 950174 The surface shape of each concave and convex part is concave or convex. Therefore, the function of layer 3 has a function of a plurality of microlenses. On the surface of the low refractive index layer 2 of the functional layer 3, the second electrode 4 When a plurality of concave concave ridges are formed on the side, the functional layer 3 functions as a plurality of concave lenses for the light-emitting layer 5. On the surface of the low-refractive-index layer 2 of the functional layer 3, a complex number is formed on the side of the low-refractive-index layer 2 In the case of a prominent convex surface (refer to Fig. 1), the functional layer 3 has a function of a plurality of convex lenses for the light-emitting layer 5. Thus, since each of the parts has a lens function, the effect of scattering, refraction, and concentrating can be achieved. It is expected to improve light efficiency. 8. The concave or convex surface is preferably a hemispherical surface. Due to the concave or convex surface, scattering can be achieved: spherical surface is expected to improve light harvesting efficiency. As the deformation is made, it is also possible to form a flat surface of each uneven portion. For example, the surface of each concave and convex portion is composed of a plane of the bottom surface of the plurality of pyramids. In the case of the change of the double-folding, the shape of the above-mentioned concave and convex portions can also be irregular, and it is preferable that the fine mutual irregularities are good. In the optical property, the wavelength dependence is exhibited. If the shapes of the respective concavo-convex portions are irregular, the wavelength dependence on the characteristics of the acquired light can be made small. ^ On the substrate, a plurality of financial EL elements I m are formed in the (four) spectrum, and the spectrum of the light of the device can be reduced to reduce the inverse of the mainly transmitted light to form a predetermined shape. For example, the red light is mainly transmitted through the ❹ 321 321 152 10 200950174, and the concave and convex portions are different from the blue color. The shape of each of the concave and convex portions that the horse mainly transmits is a coin-shaped method and a group of refractive index layers and a machine. The manufacturing method of the EL 70-piece 1 is at least a low-order product: > The first electrode, the light emission, and the refractive index of the second electrode functional layer i n2^, the refractive index n of the first electrode, and the organic electric field of the following formula (3) =::::=refractive index n3 is satisfied. * 1 _ _ Λ ^ (3) The concave core includes * a plurality of steps of forming a low refractive index layer having a height of (1) 5 #111 to 1 low refractive index per part; forming a low refractive index 已 (4) On the surface of the (4) 16 & material of the functional layer, a step of coating the electrode containing 1 i: a step of forming a functional layer to form a functional layer; forming; simultaneously giving a step of # 乂, · θ; and a step of forming a second electrode Sound: A method of manufacturing an organic EL element of a threshold, in which a first electrode is formed in the first electrode. The low-refractive-index layer is made of a transparent material that can be formed into an organic material. It can also be a soft board. For example, it can be a hard board and can be an integral sub-film formed by a laminate. A tree made of a plastic sheet or a polymer film is suitable. The first film is, for example, the light-emitting layer 5 and the hole coating method described later, and the time ττ such as the force Q f is preferably insoluble in the coating liquid of the household 321152 11 200950174. Specifically, for example, low-density or high-density polyethylene, ethylene-diene copolymer, ethylene-butene copolymer, ethylene-hexene copolymer, ethylene-octene copolymer, ethylene _norbornene copolymer δ 4Before & $ DM〇N copolymer (dmon is dimethano octahydro naphthalene; abbreviation for dimethyl bridge octadecyl naphthalene.), polypropylene, ethylene _ vinyl acetate copolymer, ethylene - Polyolefin resin such as methacrylic acid 曱 _ copolymer, ionomer resin resin; polyethylene terephthalate, polystyrene carboxylic acid, polyethylene naphthalate, etc. Ester resin; nylon 6 nylon 6'6, m-diphenylene diamine-adipic acid condensed polymer; polyamine fluorenyl propyl iodide and other acid amine resin; polydecyl acrylate vinegar, etc. Acrylic tree 曰 曰 'polyphenylene bound, styrene-acrylonitrile copolymer, styrene-propylene 1 guess a dilute copolymer, polyacrylonitrile and other styrene-acrylonitrile tree 曰 曰 vinegar & Hydrophobized cellulose resin such as cellulose or cellulose diacetate; polychlorinated ethylene, polyvinylidene gas, polyvinylidene fluoride Halogen-containing resin such as polytetrafluoroethylene; # 7 ^ ^ ^ vinyl alcohol, ethylene-vinyl alcohol copolymer, cellulose derivative, hydrogen bonding resin; polycarbonate resin, polysulfone resin, polyethersulfone tree Lunar New Year (four) _ Shu Yue, polyoxymethylene (ΡΡ0) resin, poly 曱 Ρ (Ρ Μ Μ Μ 树脂 树脂 树脂 树脂 树脂 树脂 树脂 树脂 树脂 3 3 3 3 3 3 3 3 3 3 3 3 3 3 3 。 。 。 。 。 。 Among the above resins, a resin having a glass transition temperature Tg of 150 ° C or more is preferable, and a resin of 18 (TC or more is preferable, and the resin having a glass transition temperature Tg of 150 ° C or more is preferable. It is preferable that the resin is 20 or more. The low refractive index layer may also contain a high gas barrier member which is hard to pass through oxygen and water vapor contained in the surrounding environment of the organic EL element, for example, by gold 12 321152 200950174, Metal nitride, metal carbide, and metal oxynitride: an inorganic (tetra) inorganic layer, an inorganic layer, and an organic mixed layer, etc., are preferably used, and specific examples thereof include, for example, Dioxide: a combined film layer of oxide (ΙΤ0), nitriding, nitrogen emulsified zinc oxide, indium tin, etc., and Qian 4 cut, oxygen nitrogen cut, and the film layer is better, and the oxygen layer is cut. The thin film layer formed by the formation of the milk vaporization second is more preferable. Among the examples satisfying the formula (2), the low refractive index 2 and the refractive index of the first electrode 4 are preferably selected to have a low refractive index when the composition is :===Γ The refractive index of the rate layer is the value of the refractive index of the entire low refractive index layer. The refractive index η3 of the luminosity layer is determined by the composition of the low refractive index layer, for example, when it is glass, it is about 15, and when it is polycarbonate, it is 158, and when it is quinone, it is 149 when it is The polyether is 165, and in the case of polyethylene naphthalate, it is 1.50. As for the method of forming a plurality of concave and convex portions, for example, an imprint method (pressure floating processing method), a lithography method , (4), the method of forming the concave-convex structure by the method of the tool (4) having the unevenness, the method of forming the uneven structure by the self-organization, etc., and the embossing method is used for the formation of the uneven structure through the design. The lithography method and the secret method are preferred. For example, in the imprint method, since the mold having a plurality of irregularities formed on the surface is directly pressed on the film, the surface shape of the mold can be transferred to the low refractive index layer. After the lithography technique, for example, coating the photocurable resin with 321152 13 200950174, the photo-selective irradiation is then performed on the coated film, and after the development, the coated film can be selectively removed. The surface portion can be obtained by forming a plurality of irregularities on the surface. a refractive index layer. For example, coating a photoresist on a glass substrate. After selectively removing the coated film, a mask having a plurality of holes formed thereon may be formed on the surface of the glass substrate, and further wetted by dryness. After removing the surface of the glass substrate selectively and selectively, a glass substrate having a plurality of irregularities can be obtained to obtain a low refractive index layer. The dry etching method can be used to remove the surface of the glass substrate and the resin film. Therefore, a low refractive index layer can be obtained. <Functional layer> In the functional layer, the light transmittance in the visible light region is high, and in the step of forming the EL element, the change is not applicable. It may be soft. The functional layer may be composed of, for example, an inorganic polymer, an inorganic-organic hybrid material, or the like. The inorganic-organic hybrid material may contain a compound in which inorganic and organic compounds are formed in a molecular layer, and the inorganic substance is dispersed in an organic compound to form a mixture. If the difference between the refractive index of the functional layer and the refractive index of the transparent electrode is small, since total reflection can be suppressed, it is preferably 丨.75 or more. In terms of ease of the process, the functional layer is preferably formed by coating a coating liquid containing a material capable of forming a functional layer. After the coating liquid is applied onto the low refractive index layer on which a plurality of uneven portions having a height of 0.5 #m to 1〇〇#111 have been formed on the surface, the coating liquid can be filled in the unevenness of the low refractive index layer, and then When hardened, it is easy to obtain a functional layer in which a plurality of concave and convex portions having a height of 〇5_ to 100#m have been formed. Since such a coating method is used, the surface of the functional layer 3 on the side of the first electrode 4 can be formed flat. The coating liquid may be 321152 14 200950174 as a solution 'may also be a dispersion, and an active agent, a adhesion enhancer, a crosslinking agent, an organic solvent, and an interface product may be required in accordance with the requirements. As an example, for example, the agent may be exemplified. A liquid-group aromatic monomer thermoplastic resin dispersed in a liquid, an organic polymer, and a group of thermosetting monodisperse dispersed high-refractive-nose in a high-nose particle containing a product or a photocurable monomer The meter = # becomes a material that can form the functional layer and then hardens. ..., after drying, pressurization, etc., the functional layer may be used, and there is a high-resistance member which is difficult to pass through the oxygen emulsion contained in the surrounding ring of the organic rainbow element, and the water gas. The material to be used is, for example, an inorganic layer formed of an inorganic substance such as a metal, a metal oxide, a gold metal, or a gold alloy; a laminate of a layer and an organic layer, or an inorganic-organic mixed inorganic machine layer, preferably Thin film layer and stable in air, ° as a flawless dioxide dream, oxidation, titanium dioxide, oxygen: for example: emulsifying shop, tin oxide, zinc, copper tin oxide, nitriding, nitriding Dream, titanium carbide, gas and a combination film layer of these. Preferably, the thin film layer formed by nitriding, nitrogen, and oxygen emulsification is preferably a thin layer of chlorinated stone formed by oxygenated fossils, which is more preferable under the limitation of formula (1) and formula (2). Among the examples of the refractive indices of the machine 2 and the first electrode 4, the refractive index of the refractive index layer is such that the relationship of the formula (1) and the formula (2) can be satisfied. f energy layer: good. When the functional layer is composed of a plurality of members: the refractive index of the entire functional layer. The refractive index of the b layer is *321152 15 200950174 The refractive index n2 of the functional layer is determined by the constituent material constituting the functional layer, for example, 175 to 2 Å in the case of the inorganic polymer of the Shixi, dispersing Ti in the polymer. When the mixture of 〇2 is 1, 8 to 2 〇. <First Electrode> * The first electrode 4 of the present invention can be made of a film exhibiting light transmissivity and conductivity. For example, it can be composed of a metal oxide film, a metal thin film or the like, and f is an example thereof. Such as: indium oxide, zinc oxide, tin oxide, antimony tin oxide (Indium Tin 0xide: _, _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ _ Further, a film of 1T, IZ, or tin oxide is preferred. As the first electrode 4, an organic transparent conductive film such as polyaniline or a derivative thereof, polybenzazole or a derivative thereof may be used. The thickness is suitably set after considering light transmittance and conductivity, and is generally about 1 〇 to 1 〇 _, and preferably 2 〇 (10) to 1 # m, more preferably 5 〇 nm to 500 nm. Examples of the method for forming the first electrode include a vacuum deposition method, a frequency method, an ion plating method, an electric ore method, etc. The refractive index n1 of the first electrode depends on the constituent material constituting the first electrode, for example, When TM is 2.0, when it is IZ〇, it is 19 to 2 Å, and when it is an organic transparent conductive film such as polythiophene or a derivative thereof, it is about 17 <Curtain injection layer> As a hole injection material constituting the hole injection layer, for example, a phenylamine compound, a starburmer (a dendritic structure having a radiation phase), a dragon compound (4) Compounds, oxides of vanadium oxide, molybdenum oxide, cerium oxide, aluminum oxide, amorphous carbon, polyaniline, 321152. 16 200950174 Polythiophene derivatives, etc., can be formed by coating, for example, on the first electrode. The hole injection layer is formed into a hole injection layer, and examples of the method for applying the coating liquid include a spin coating method, a casting method, a micro gravure coating method, a gravure coating method, and a strip coating method. Roll coating method, wire bar coating method, dip coating method, spray coating method, screen printing method, soft printing method, lithography method, inkjet printing method, etc. <Light-emitting layer> The organic matter of the light and/or the lining is composed of or contains the organic matter and the dopant. The dopant may be added for the purpose of, for example, improving the luminous efficiency or changing the wavelength of the luminescent light. The organic substance used on the luminescent layer may be low. Minute The luminescent material constituting the luminescent layer is exemplified by the following. Examples of the luminescent material of the dye include a cyclopentamine derivative, a tetraphenylbutadiene derivative compound, and the like. Phenylamine derivatives, oxadiazole derivatives, pyrazoloquinoline derivatives, stilbene benzene derivatives, stilbene aromatic hydrocarbons ((115 7711 & "16116) derivatives, 1» 嘻 derivatives a porphin ring compound, a pyridine ring compound, a per i none derivative, a pery i ene derivative, a polythiophene derivative, an oxadiazole dimer, and a pyrazoline dimer. Examples of the light-emitting material of the metal complex compound include Ir (铱), Pt (platinum), A1 (aluminum), Zn (zinc), Be (铍), etc., or Tb (铽) in the center metal. a rare earth metal such as Eu (铕) or Dy (镝), a metal complex compound having a oxadiazole, a thiodazole, a phenylpyridine, a phenylimidazole, a quinoline structure or the like in the ligand, for example, From the indium complex compound, platinum coordination 321152 17 200950174 compound and other triple-excited state luminescence metal coordination compound, Ming 喧 配 配 钱 、 、 笨 笨 笨 笨 笨 笨 笨 笨 笨 笨 笨 笨 笨 、 、 、 、 a bismuth, a benzamidine zinc complex, an azomethyl zinc complex, a zinc porphyrin complex, an iridium complex, and the like. Examples of the luminescent material of the street oysters include: poly(p-phenylene ether) = biological, (tetra) phenanthrene derivatives, poly-p-polyacetylene derivatives, polyglycosides, and luminescence of the above-mentioned hue. = B-selling organisms, etc., to materialize macromolecules. 4 or a metal complex compound luminescent material such as the above luminescent material, stilbene aromatic hydrocarbon derivative, 2 cut materials, can be exemplified 'polyvinyl carbazole derived plate heart azole and his biology, and Among them, poly-derivatives of polymer materials, poly-W organisms, and the like are used. Or poly* derivatives, etc. are preferred. Oxazol, poly(p-phenylene derivative) - A coumarin derivative, an anthrone derivative, a fragrant organism, a poly derivative, etc., on a material that emits green light. ^(4), polystyrene derivative, polyg derivative, etc. are preferred. Poly(p-phenylene terephthalate) of a molecular material On a material that emits red light, a compound can be exemplified, and such polymers are: aroma, a derivative, a phenanthrene, a poly(tetra), and the like. Among them, ^ 埽 埽 derivatives, poly acetamidine derivatives, poly. The t-phene derivative The molecular material is agglomerated on the dry material that emits white light, and is also preferred. The red light materials are mixed and used. ^ A plurality of materials which emit blue light, green light, and various components which respectively emit the above-mentioned materials of 200950174 blue light, green light and red light in one molecule are used for white light emitting materials, for example, materials of various colors: As the monomer, a polymer obtained by polymerization is used as a material for emitting white light: an element which emits white light can be formed by laminating a plurality of layers which can emit different luminescent colors. As the dopant, for example, a flower derivative, a coumarin derivative, a rubrene derivative, a ruthenium, a tetragonal ring (referred to as ο)

SqUarliUm) derivatives, exoline derivatives, styrene derivatives, naphthacene derivatives, pyrazolone derivatives, decacycloolefin, phenoxazinone (Ph (10) xaz (tetra)) and the like. The thickness of such a light-emitting layer is usually about _ to 2, OOOnm. The film forming method of the organic light-emitting layer may, for example, be a method of applying a coating liquid containing a light-emitting material to the hole injection layer 7, a vacuum film, a transfer method, or the like. The solvent which is a coating liquid containing a light-emitting material may be a liquid which can dissolve the light-emitting material, and examples thereof include (IV), a methylene chloride field, a chlorine solvent such as chlorsamine, and an ether solvent such as tetrahydrofurfuryl. Toluene, secret brewing, etc., such as ketone solvents such as stimulant, propionate, methyl ethyl ketone, ethyl acetate, butyl acetate, ethyl acetate (Ethyiceii〇sive acetate), etc. Ester solvent. The method of applying the coating liquid of the luminescent material to the spine, for example, a tumbling coating method, a casting method, a micro coating method, a roll coating method, a bar coating method, a gravure coating method, and a strip coating method. , spraying method, nozzle dip coating method, slit coating method, wool screen printing method, soft printing method, flat reading method, gravure printing method, thousand printing method, reverse printing method, spraying 321152 19 200950174 Coating method such as ink printing method. The coating method is preferably a gravure printing method, a screen printing method, a flexographic printing method, a lithographic printing method, a reverse printing method, or an inkjet printing method. Meanwhile, in the case of sublimating low molecular compounds, vacuum evaporation can be used, and only a desired luminescent layer can be formed by laser (laser) transfer or thermal transfer. In the present embodiment, the second electrode 6 has a function as a cathode, and as a material of such a second electrode, a material having a small work function and being easily injected into the light-emitting layer is preferable. At the same time, a material with high conductivity is preferred. Specifically, 'metals such as alkali metals, alkaline earth metals, transition metals, and Group W metals can be used, and more specifically, such as: bell, nano, n planer, bismuth, town, calcium, strontium, barium, ing, sharp , vanadium, zinc, antimony, bismuth, antimony, bismuth, pin, bismuth, mirror, etc., or more than two of the above metals, or more than one of these metals, with gold, silver, titanium, Two: one or more alloys of tungsten and tin, or five layers of graphite or graphite. As for the example of the alloy, it can be exemplified by magnesium alloy, magnesium-indium alloy, town-aluminum alloy, indium-silver alloy, collar _^ human mouth fish, lithium aluminum alloy, lithium-magnesium alloy, lithium — Marriage & Golden Order 1 Lu alloy. When light is to be obtained from the second electrode, the second electrode must be a transparent second electrode that is so transparent that it can be composed of a laminate of the film-forming electrical metal oxide or the guide film formed as described above. . In the first embodiment of the wind, the combination of the low refractive index layer 2, the functional layer 3, and the first electrode 4 is a glass substrate, an inorganic polymer, and (10) is preferably 321152 20 200950174, :::: fat, inorganic polymer And ίτο is better. ❹ ❹ and the light-emitting layer 5 are disposed in the EL element ', although the composition of the EL element i of the hole injection layer 7 is between the two electrodes 4 and the second electrode 6, but the first to the first of the organic components The composition shown in the figure. The following examples are explained. Any one of the element or the cathode of the electrode and the second electrode is required to be transparent. The description of the polarity of the anode and the second electrode is not particularly limited to the first electric power. For example, an example of the composition of a thin piece of thin. At the same time, it is made of a resin on a substrate such as glass. When the layer 2 is used, the low refractive index layer may be disposed between the anode and the cathode of the t@5彳f, and at least one layer of the light emitting layer may be disposed between the entangled dipole and the cathode, and/or 5 A layer different from the first layer or a layer of a plurality of layers. As the Zen between the cathode and the light-emitting layer, for example, an electronic note can be cited.

Si;: sublayer, hole block layer, and the like. When the two layers of the electron transport layer are provided between the cathode and the light-emitting layer, the layer located near the cathode side, the 'main entrance layer, and the layer near the light-emitting layer is called the electron transport layer. The electron injecting layer is a functional layer having an efficiency of improving electron injection from the cathode. The electron transport layer is a functional layer having an improved injection of electrons from the cathode, or the electron injection layer, or from an electron transport layer closer to the cathode. The electric hole block layer has a functional layer that blocks the transportation of the hole. At the same time, it is possible to make the electron injecting layer or the electron transporting layer double as a hole block layer. As a layer provided between the anode and the light-emitting layer, for example, a hole injection 321152 21 200950174 an interlayer electrical hybrid layer, an electron block layer, etc., between the anode and the light-emitting layer, and a hole injection layer and electricity When the two layers of the hole transport layer are used, the layer located near the anode side is called the hole injection layer', and the layer located near the side of the light-emitting layer is called the hole transport layer. The hole injection layer is a functional layer having an efficiency of improving the injection of holes from the anode. The hole transport layer is a ship layer having improved (9) polling layer injection holes from the anode, or the hole injection layer, or from the 1 匕 anode. Electronic block

The layer is a functional layer with a neon electronic transfer. The hole injection layer or the hole transport layer can double as an electron block layer. The electric m layer and the hole injection layer are collectively referred to as a charge injection layer. The electron transport layer and the hole transport layer are collectively referred to as a charge transport layer. One of the specific examples of the layer composition of the organic EL element is shown below. a) anode/hole transport layer/light-emitting layer/cathode b) anode/light-emitting layer/electron transport layer/cathode c) anode/hole transport layer/light-emitting layer/electron transport layer/cathode d) anode/charge injection layer/ Luminescent layer/cathode

e) anode/light-emitting layer/charge injection layer/cathode f) % pole/electric street injection layer/light-emitting layer/charge injection layer/cathode g) anode/charge injection layer/hole transport layer/light-emitting layer/cathode h) anode / hole transport layer / light-emitting layer / charge injection layer / cathode i) anode / charge injection layer / hole transport layer / light-emitting layer / charge injection layer / cathode j) anode / charge injection layer / light-emitting layer / charge transport layer / Cathode k) Anode / luminescent layer / electron transport layer / charge injection layer / cathode 22 321152 200950174 l) Anode / charge injection layer / luminescent layer / electron transport layer / charge injection layer / cathode m) anode / charge injection layer / hole Transport layer / luminescent layer / charge transport layer / cathode η) anode / hole transport layer / luminescent layer / electron transport layer / charge injection layer / cathode 〇) anode / charge injection layer / hole transport layer / luminescent layer / electron transport The layer/charge-injecting layer/cathode (the symbol "/" in this case is a layer of the adjacent layer of the holding mark "/". The same applies to the following.) The organic EL device of the present embodiment may have two layers. The above luminescent layer. Specific examples of the organic EL element having the two-layer light-emitting layer include P) anode/charge injection layer/hole transport layer/light-emitting layer/electron transport layer/charge injection layer/electrode/charge injection layer/hole transport Layer composition of layer/light-emitting layer/electron transport layer/charge injection layer/cathode_. As for the organic EL element having three or more light-emitting layers, when (electrode/charge injection layer/hole transport layer/light-emitting layer/electron transport layer/charge injection layer) is a repeating unit, More than q) the anode/charge injection layer/hole transport layer/light-emitting layer/electron transport layer/charge injection layer/repetition unit/repetition unit cathode repeat unit layer composition. In the above layer composition {> and q, each layer other than the anode, the electrode, the cathode, and the light-emitting layer can be removed as required. 321152 23 200950174 The bottom emission type organic EL element which obtains light from the substrate 8 is a layer which is disposed on the substrate 8 in a completely transparent layer on the basis of the light-emitting layer. A so-called top emission type organic EL device which obtains light from the opposite side of the substrate with reference to a light-emitting layer to be described later is disposed on the layer opposite to the substrate with a transparent layer as a reference based on the light-emitting layer. In the organic EL device, an insulating layer having a film thickness of 2 nm or less may be adjacently provided on the electrode to further improve adhesion to the electrode or to improve injection charge from the electrode, or to insert a thin buffer layer at an interface adjacent to the respective layers. To improve the adhesion of the interface or prevent mixing. Ο The specific composition of each layer will be described below. At the same time, since the light-emitting layer 5 and the hole injection layer 7 have been described above, the overlapping description will be omitted. In the anode and/or the cathode, since the first electrode or the second electrode described above can be used, the overlapping description will be omitted. <Curtain transport layer> As the hole transporting material constituting the hole transport layer, for example, polyvinyl carbazole or a derivative thereof, polydecane or a derivative thereof, and a fragrance on a side chain or a main chain 可 may be mentioned. a polyoxane derivative of a amine, a pyrazoline derivative, an aromatic amine derivative, a stil bene derivative, a triphenylenediamine derivative, a polyaniline derivative or a derivative thereof, a polythiophene or a derivative thereof, a polyarylamine or a derivative thereof, a polypyrrole or a derivative thereof, a poly(p-phenylene vinyl) or a derivative thereof, or a poly(2,5-thienylethylene) or a derivative thereof Wait. Among these hole transport layers, as the hole transporting material, polyethylene carbazole or a derivative thereof, polydecane or a derivative thereof, and an aromatic amine compound group in a side chain or a main chain are used. Oxylkane derivative, polyaniline or its 24321152 200950174 derivative, polythiophene or its derivative, polyarylamine or its derivative, poly(p-phenylene vinyl) or its derivative, or poly(2, 5 a hole transporting material of a polymer such as a thienylethylene or a derivative thereof, and a polyvinyl carbazole or a derivative thereof, a polydecane or a derivative thereof, and an aromatic amine in a side chain or a main chain A polyoxyalkylene derivative or the like is preferred. In the case of a low-molecular hole transporting material, it is preferred to use a polymer binder dispersed therein. As for the film formation method of the hole transport layer, in the low-molecular hole transport material, a method of forming a film by a mixed solution with a polymer binder may be mentioned; in a polymer hole transport material; A method of forming a film by a solution can be mentioned. The solvent to be used for film formation from a solution may be any solvent which can dissolve the hole transporting material, for example, a chlorine solvent such as chloroform, dichloromethane or dichloroethane, or an ether solvent such as tetrahydrofuran or the like. An aromatic hydrocarbon solvent such as benzene or xylene; a ketone solvent such as acetone or mercaptoethyl ketone; or an ester solvent such as ethyl acetate, butyl acetate or ethyl cellulose acetate. ❿ As a method of forming a film from a solution, for example, a spin coating method, a casting method, a micro gravure coating method, a gravure coating method, a strip coating method, a roll coating method, a wire bar coating method, a dip coating method, and a spray coating method Coating methods such as a method, a screen printing method, a soft printing method, a lithography method, and an inkjet printing method. As a mixed polymer binder, it is preferable that the carrier is not hindered from being extremely poorly charged, and the absorption of visible light is weak. As the high molecular weight binder, for example, polycarbonate, polyacrylate, methyl acrylate, polymethyl methacrylate, polystyrene, polyvinyl chloride, polyoxymethane or the like can be mentioned. 25 321152 200950174 As the thickness of the hole transport layer, the optimum value varies with the materials used, and the drive voltage and luminous efficiency are selected to be moderate values, but at least the thickness does not produce pinholes, such as too thick At this time, the driving voltage of the element will be lowered. Therefore, the thickness of the hole transport layer is, for example, from 1 nm to 1 #m, preferably from 2 η π to 500 nm, more preferably from 511111 to 2 〇〇 nm. <Electron injection layer> As an alloy of the composition of the electron injecting layer, which is an alkali metal, an alkaline earth metal, or an alloy containing one or more of the foregoing metals, or the aforementioned metal Oxides, complexes and carbides, or mixtures of the foregoing, and the like. As for the alkali metal or its oxide = carbonization = for example, · clock, nano, unloading, recording, oxidation, fluorine: 匕: = nano, sodium fluoride, potassium oxide, potassium fluoride, oxidation two W, gasification Broken acid clock, etc. As the chemical, the dentate and the carbide, for example, m, emulsified money, gasified town, oxygen, fluorinated, cerium oxide, and the like are mentioned. , rolling, i-recording, magnesium carbonate, etc. The electron injection layer can also be a laminate of shellfish and oxide. As for the specific example of the laminate, a layer of electron injection layer can be formed by enamel, such as LiF/Ca. ",, and, sputtering, printing, etc." The thickness of the electron injecting layer is preferably from 1 nm to 丨. Partial. As for <electron transport layer> as an electron wheel constituting the electron transport layer Sending the wrong two-streak derivative, simmering dimethyl sulphate or its exemplified by: naphthalene awake or its ejaculation, technology or its, or its derivatives, its derivatives, the first network derivative, four mouse 蒽A metal complex compound, polyquinoline or a derivative thereof, or a metal complex compound of the dimethyst or a base thereof, a 32JJ52 26 200950174 diphenolphthalein derivative, or 8-hydroquinoline or a derivative thereof Quinolin or a derivative thereof, polyfluorene or a derivative thereof, etc. Among them, as an electron transporting material, an oxadiazole derivative, benzoquinone or a derivative thereof, an anthracene or a derivative thereof, or 8 a metal complex compound of hydrogen quinoline or a derivative thereof, polyquinoline or a derivative thereof, polyquinoxaline or a derivative thereof, polyfluorene or a derivative thereof, preferably 2_(4_linked base) _5 - (4-tert-butylphenyl)-1,3,4-oxadiazole, benzoquinone, anthracene, tris(8-hydroxyquinoxaline) aluminum, polyquinoline is more preferred. Fig. 2 is a schematic view showing an organic EL element 11 according to another embodiment of the present invention. The organic EL element u of the present embodiment is at least a functional layer 13, a transparent first electrode 14, a light-emitting layer 15, and a second electrode. An organic electroluminescent element composed of a sequential layer, wherein a plurality of concave and convex portions having a height of 〇.5/zm to 100m can be formed on the surface of the functional layer 13 opposite to the second electrode 14 ! The refractive index n1 of the electrode 14 and the refractive index of the functional layer 13 are the same as those of the organic EL element 11 of the above-described embodiment, and may be provided between the τ electrode 14 and the second electrode 16 as well. The layers of the luminescent layer 15 are different, and as described above, a plurality of layers can be formed. The organic germanium element 11 of the present embodiment is provided adjacent to the surface of the substrate 18 in the order of the second electrode 16, the hole injection layer 14, the light-emitting layer 15, the first electrode 14, and the functional layer 13. The organic EL element n of the present embodiment is a so-called top emission type element which can emit light from the light-emitting layer 15 and can be externally obtained by transmitting the first electrode 14 and the functional layer 13. 321152 27 200950174 The substrate 18 of the present embodiment may be transparent or opaque, for example, a plate body which may be composed of the same material as the low refractive index layer 2 described above. The first electrode 14 of the present embodiment can also use the ith electrode of the above-described embodiment, and is similar to the transparent second electrode 6 described in the "D" mode. ::: From an alkali metal, an alkaline earth metal, a transition metal And a laminate of a film of the ΠΙ-Β 金属 metal, and a film of a conductive organic bismuth compound (IV) electrically organically laminated. At the same time, the second electric = transparent in the present embodiment may be opaque, and the electrode 4 or the second electrode 6 of the above embodiment may be used. At the same time, the surface of the second electrode 16 may be provided with a reflective layer composed of a member which can reflect light such as metal. The functional layer 13 of the present embodiment is the same as the machine = 3 in the above embodiment, and the description thereof will not be repeated. The functional layer of the present embodiment can be bonded to the i-th electrode 12 by forming a concave portion f by the same method as the functional layer 3 of the above-described embodiment. At the same time, it is also possible to form a plurality of concave and convex portions on the functional layer 3 in the same manner as the above-described method of forming the low refractive index layer 2, and then attach it to the first electrode, and also to the first electrode 14 Formed directly on the top. Organic EL element u composed in this way, due to the first! Since the refractive index difference between the electrode u and the function «13 is small, the reflectance of the interface between the functional layer 13 and the second electrode can be lowered, and total reflection can be suppressed. Therefore, light can be efficiently incident from the ^1 electrode 14 into the functional layer 13. At the same time, since a plurality of concave and convex portions having a height of 〇.5#111 to 1〇〇# can be formed on the surface of the functional layer 13, the light which can be incident on the functional layer U as described above is 321152 28 . 200950174 The effect is obtained outside. As described above, the light emitted from the light-emitting layer 15 can be efficiently transmitted to the first electrode 14, the functional layer 13, and the air in order, and the light-acquisition efficiency can be improved. Fig. 3 is a schematic view showing an organic EL element 21 according to another embodiment of the present invention. The organic EL element 21 of the present embodiment is a top emission type element in which the low refractive index layer 22 is further added to the organic EL element n of the embodiment described in the second embodiment, and the organic EL of the above embodiment. Since the element 11 is different only in the low refractive index layer 22, only the low refractive index layer 22 will be described, overlapping the description.

The low refractive index layer 22 of the present embodiment functions as a sealing film for blocking water, oxygen, or the like on the organic EL member 21, and is, for example, a metal, a metal oxide, a metal nitride, a metal carbide or An inorganic layer formed of a metal oxynitride or the like, or a layer in which the inorganic layer is combined with an organic layer, or an inorganic-organic mixed layer or the like is suitable. As for the inorganic layer, it is preferable to use a film layer and 10 amps in air, and specifically, for example, cerium oxide, aluminum oxide, titanium white, oxidized steel, vaporized tin, titanium oxide, zinc oxide, indium tin oxide. 1, a turn-over, tantalum nitride, tantalum carbide, niobium oxynitride, and a combined film layer of these. Further, a thin film layer formed of aluminum nitride, tantalum nitride or hafnium oxynitride is more preferable, and a thin tantalum layer formed by oxynitride is more preferable. The low refractive index layer 22 covers the second electrode 16, the hole injection layer 17, the light-emitting layer 15, and the first electrode 14 by a vacuum deposition method, an upsetting method, or a lamination method in which a metal thin film is heat-pressed. And the functional layer 13 is formed. The refractive index n3 of the low refractive index layer 22 of the present embodiment satisfies the above-mentioned 29 321152 200950174 formula (2). Therefore, similarly to the organic EL element shown in the first embodiment, the light emitted from the light-emitting layer 15 can be efficiently transmitted to the second electrode 14, the functional layer 13, the low refractive index layer 22, and the air in order. Improve the efficiency of light. The organic EL device of the above-described embodiments, the use of the elementary device of u, and the plurality of organic EL elements of the above-described embodiments can be used as an illumination device, a planar light source, a segment display device, and a dot matrix display. The light source of the device, and the backlight of the liquid crystal display device, are particularly suitable as illumination devices. When the organic rainbow element of the present embodiment is used as a planar light source, the cathode and the cathode are seen as a weight == from the direction of the lamination direction. At the same time, 'in the light source that constitutes the segment display element, and fortunately: the organic light-emitting element of the light-emitting layer has a mask for opening the light-transmitting window in a predetermined pattern on the surface of the planar light source, so that It is necessary to form a pattern in which the organic layer of the extinction portion is extremely thick and substantially emits light, and at least one of the anode and the cathode forms a predetermined pattern. By forming an organic EL 7L member that can emit a predetermined pattern by such a method, a plurality of electrodes can be selectively applied as a line, and a segment type display for displaying a number, a character, or a simple mark can be made. Device. When the light source of the dot matrix display device is to be formed, the anode and the cathode are respectively formed in stripes, and are arranged so as to be perpendicular to each other as viewed from the direction of the stacking direction. If you want to create a dot matrix display device with partial color display and extra-luxury display, you can use a method that can separate the luminescent materials of the same luminescent color S and use color filters and fluorescent 321152 30 200950174 conversion. Filters and other methods can be used. The dot matrix display device may be a passive drive or an active drive combined with a TFT or the like. These display devices can be used as display devices such as computers, televisions, portable terminals, mobile phones, car navigators, and video camera viewfinders. Further, the planar light source is self-illuminating and thin, and can be applied as a backlight of a liquid crystal display device or a planar illumination device. At the same time, as long as a flexible substrate is used, it can also be used as a curved light source or display device. [Example 1] ® <Production of Substrate> A transparent positive photoresist material having a refractive index similar to that of a glass substrate (refractive index of 1·52) by a spin coater (trade name, manufactured by Tokyo Ohka Kogyo Co., Ltd.) "TFR970", refractive index of 1.59) was opened on a glass substrate of 5 cm x 5 cm, and a film having a thickness of 5 #π was formed, and then heated on a hot plate for a second. A 50 mj/cm2 ί line was irradiated with a blister having a circular permeable field having a diameter of 8.5/nn. After developing at room temperature with 〇55% K〇H aqueous solution (8 sec), it was heated on a hot plate at 22 (TC for 1 minute, and then refluxed to form a height on the surface of the photoresist film.不5 to 4. The irregular concavo-convex structure (formation of a low refractive index layer). A high refractive index coating film forming solution having a refractive index of 1.8 on a concave-convex structure (manufactured by RASA Industries, trade name "RASA TI") After that, the center line roughness Ra of the outermost surface of the functional layer is 2. 8 nm, and then 12 〇 on one side. (: heating the substrate, while ιτο (refractive index 20) is sputtered into the film on the functional layer with a strip of 5 cm x 5 cm and a film thickness of 3 Å (DC sputtering method, film formation pressure 0.25 Pa, power 25.25kW) 321152 31 200950174 (formation of transparent electrode). Then it is treated with 2Q (rc^ 4 () minutes of annealing (annealing) in the towel. Use 5 〇 strong alkaline cleaner, cold water, 5 ( After the TC's warm water is ultrasonically cleaned, it is taken out from the warm water of the step, and then it is made into a towel. _ 进行 纯 纯 pure cleaning for 2G minutes, can be obtained The first electrode of the present invention. &lt;Production of organic EL device&gt; Poly(3,4)ethylenedioxythiophene/polyphenylene-binding acid (manufactured by Starck Co., Ltd., trade name: AI4) using a filter having a 〇.45 μm diameter After the suspension of 〇83) was filtered, the filtrate was applied onto the cleaned substrate by spin coating to form a 65 mn thick film. After heat treatment in a hot plate for 2 to 5 minutes on a hot plate in the atmosphere, The hole injection layer was formed. Then, a wpi33 S of Sumeiti〇n, which is a material of a white knives and a sub-organic EL luminescent layer, was dissolved in benzene to form a polymer solution of 0.8% by mass, which was spin-coated. The knife sputum is coated on the substrate on which the hole injection layer has been formed to form a film of a thicker thickness. Then, after heat treatment on a hot plate at 13 (rc for 3 〇/knife clock), a luminescence is formed. The substrate on which the light-emitting layer has been formed is introduced into a vacuum evaporation machine so as to be perpendicular to the pattern of IT〇 as a cathode

Ba^Ab was sequentially vapor-deposited to a thickness of 1 〇 nm and 1 〇〇 nm and formed into a strip shape of 5 cm x 2 cm, that is, a second electrode was formed. In the step of forming the second electrode, the metallization of the metal is started after the degree of vacuum reaches 1x1 〇 4 Pa or less. Finally, in the inert gas, the vertical portion of the first electrode and the second electrode is covered with a glass plate as a center, and the four sides are covered with a photocurable resin, and then the photohardenable resin is cured by uv irradiation to form an organic EL element 0 321152 32 200950174 (Comparative Example 1) &lt;Production of Substrate&gt; A ΙΤ0 film was formed on the glass substrate (refractive index L 52) of 5 cm x 5 cm in the same manner as in Example 1. <Production of Organic EL Element> An organic EL element was formed on the substrate on which the ITO film was formed in the same manner as in Example 1. &lt;Evaluation of Light-Emitting Characteristics of Organic EL Element&gt; © The light-emitting characteristics of the organic EL element obtained in Example 1 and Comparative Example 1 were evaluated. The front light-emitting luminance when a voltage of 8 V was applied to the entire device was measured. The brightness meter is using BM-8. The luminance of the organic EL element in Comparative Example 1 was 4,865 d/m 2 , and the organic EL element in Example 1 was 5,5,785 d/m 2 . Thus, it was confirmed that the organic electroluminescence element of the present invention has the functional layer and the low refractive index layer, so that the light acquisition efficiency can be improved. (Example 2) 制作 <Production of Substrate> On a matte-finished surface of a 5 cm x 5 cm single-faced ground glass substrate (refractive index ι 52) manufactured by San and Frost Co., Ltd., which corresponds to a low refractive index layer, After the steps of (1) to (3) are repeated eight times in a sequential round of processing, a functional layer having a refractive index of 1.98 can be formed. (1) A step of spin coating a liquid for forming a high refractive index coating film having a refractive index of 18 (manufactured by RASA Industries, trade name "RASA TI"). (2) A step of heating on a hot plate at 15 (TC for 1 minute. (3) a hardening step of heating at 380 ° C for 1 minute on a hot plate. The uneven structure on the matte surface of the frosted glass substrate is rz = =1· 998, and the functional layer 33 321152 200950174 ·

Among the outermost surfaces, the line thickness Ra is 8 8 nm. Then on the side with (10). C heating the substrate, - the edge of the refractive index 2. 〇) with a band of 5cm x 5cffi and a film thickness of 3 〇〇 nm on the functional layer _ film formation (DC seam *, film formation pressure 〇.25Pa' power 〇.25kw After that, a transparent electrode having a refractive index of 2 Å was formed. Then, in the furnace, the substrate was annealed at 2 G (TC for 40 minutes to obtain a substrate with a transparent first electrode. &lt;Evaluation of light efficiency by PL&gt; 3 lining as a green polymer organic muscle luminescent material The GP country of the heart (company name) was dissolved in toluene, adjusted to a 12-fine fine polymer solution, and this solution was applied by spin coating on the cut film of the substrate obtained by the upper layer. The film thickness of the obtained coating film was m from green high. Molecularly, the luminescent layer is irradiated with ultraviolet rays of 365 nm, and then the intensity of the green light PL emitted from the back surface of the substrate is measured. The PL intensity is 3'020 (any unit), and the so-called pL is

Abbreviation for Ph〇t〇lumineSCence. After the luminescent material is excited by light (photon, coffee (4), the luminescence characteristic of the luminescent material is detected - cence). In the evaluation of the light-harvesting efficiency, X is evaluated by illuminating the pl-emitting light as EL luminescence. At this time, since the 365 nm ytterbium is irradiated on the luminescent layer, after the luminescent material is emitted, the light intensity of the entire emitted light of the substrate can be detected by the integrating sphere. (Comparative Example 2) &lt;Production of Substrate&gt; The same procedure as in Example 2 was carried out on a glass substrate (refractive index: 52) of 5 cm x 5 cm, and an IT crucible film was formed. <Application of PL evaluation light acquisition efficiency> 32Γ152 34 200950174 A green polymer organic EL light-emitting material was applied on the ITO film of the substrate obtained above in the same manner as in Example 2. After 365 nm of ultraviolet rays were irradiated from the green polymer organic EL light-emitting layer, the intensity of the green light PL emitted from the back surface of the substrate was measured. The PL intensity is 2,271 (any unit). The PL intensity obtained in Example 2 was 1.33 times the PL intensity obtained in Comparative Example 2. When the organic EL device is fabricated by using the substrate obtained in the second embodiment to produce the organic EL device, the light-receiving efficiency of the device can be improved by providing the functional layer and the low refractive index layer. 〇 [Application possibility in the industry] With the application of the present invention, an organic electroluminescence element having high light-recovering efficiency can be produced. BRIEF DESCRIPTION OF THE DRAWINGS Fig. 1 is a schematic view showing an organic EL element 1 according to an embodiment of the present invention. Fig. 2 is a schematic view showing an organic EL device ?11 according to another embodiment of the present invention. Fig. 3 is a schematic view showing an organic EL element 21 according to another embodiment of the present invention. [Description of main component symbols] 1, 11, 21 Organic EL device 2 &gt; 22 Low refractive index layer 3 ' 13 Functional layer 4 ' 14 First electrode 5 ' 15 Light-emitting layer 6 ' 16 Second electrode 7, 17 Hole injection Layer 8 substrate 35 321152

Claims (1)

200950174 VII. Patent application scope: L-type organic electric field light-emitting element is an organic optical component composed of a functional layer, a transparent electrode, a light-emitting layer and a second electrode, and is known as an organic light element. On the opposite side of the electrode of the target plane, a plurality of concave and convex portions having a height of 〇.5/zm to 1Q g1丨1 king 1 υϋ # m are formed, and the refractive index n1 of the first electrode is as described above. The folding (10) n2 of the functional layer can satisfy the following formula (1) ^ (1). n. (nl-n2)^ 〇2. The organic electroluminescent article of claim 1, wherein the low refractive index layer is the first layer of the functional layer The surface of the opposite side of the electrode is adjacent to each other, and the refractive index η of the first electrode, the refractive index of the functional layer, and the refractive index of the low refractive index layer satisfy the following formula (2)), η1 - η2 &gt; η3 (2) 〇 3 The organic electroluminescence device of claim 1, wherein the surface line average roughness Ra of the surface of the second electrode side of the functional layer is 1 〇 nm or less. In the organic electric field light-emitting element of any one of the claims 1 to 3, the arrangement interval of the concave-convex portions is 0.5/zm to 1〇〇# m ° as in the patent scopes 1 to 4 The organic electric field light-emitting element of any one of the organic electric field light-emitting elements is a concave or convex surface as described in claim 5, wherein the concave or convex surface is 7. The organic electroluminescent device according to any one of claims 1 to 4, wherein the surface shape of each of the concave and convex portions is composed of a plurality of different planes. The organic electroluminescence device of any one of the items 1 to 4, wherein the irregularities are irregular in shape. 9. A lighting device comprising any one of claims 1 to 8 of the patent application. An organic electric field light-emitting element according to any one of claims 1 to 8. 11. A method of manufacturing an organic electric field light-emitting element, The element is composed of a low refractive index layer, a functional layer, a transparent first electrode, a light-emitting layer and a second electrode, and the refractive index n1 of the first electrode, the refractive index n2 of the functional layer, and the low The refractive index n3 of the refractive index layer can satisfy the following formula (3)' ί〇. 3^(η 1-η 2)^0 · · · (3) [nl^n2&gt;n3 The system includes: forming a plurality of surfaces on the surface a step of forming a low refractive index layer having a height of 0.5 to 100 / zm; applying a coating containing a material as a functional layer on the surface of the plurality of concave and convex portions on which the low refractive index layer has been formed a step of forming a functional layer after liquid; a step of forming a first electrode; 37 321152 200950174 a step of forming a light-emitting layer; and a step of forming a second electrode. 12. A method of manufacturing an organic electroluminescent element according to claim 11 In the step of forming the low refractive index layer, a plurality of concave and convex portions are formed by an imprint method. 13. The method for producing an organic electric field light emitting device according to the first aspect of the invention, wherein Refractive index layer In the step, the surface portion of the low refractive index plate is selectively removed by a lithography technique to form a plurality of concave and convex portions. ❹ 14. The method for manufacturing an organic electric field light emitting device according to claim 11 Wherein, in the step of forming the low refractive index layer, the surface portion of the low refractive index plate is selectively removed by a dry etching technique to form the uneven portion. 38 321152